Silver and cesium diffusion dynamics at the ß-SiC Σ5 grain boundary investigated with density functional theory molecular dynamics and metadynamics.

The diffusion and release of silver-110m, a strong γ-radiation emitter, through silicon carbide in coated nuclear fuel particles has remained an unsolved topic since it was first observed 40 years ago. The challenge remains to explain why, contrary to other elements, silver is capable of escaping the ceramic diffusion barriers. The current work investigates the underlying differences in the diffusion of silver and cesium along a symmetric tilt Σ5 grain boundary of ß-SiC through accelerated density functional theory molecular dynamics simulations. The energy barriers extracted from the simulations give diffusion coefficients that are in reasonable agreement with experiment for silver (2.19 × 10(-19) to 1.05 × 10(-17) m(2) s(-1)), but for cesium the equivalent calculated coefficients for this mechanism are much smaller (3.85 × 10(-23) to 2.15 × 10(-21) m(2) s(-1)) than those found experimentally. Analysis of the simulated structures and electron densities and comparisons with the calculations of other researchers suggest that diffusion of silver and cesium in ß-SiC proceeds via different mechanisms. The mechanisms of cesium diffusion appear to be dominated by its relatively large size and repulsive interactions with the silicon and carbon atoms; ß-SiC grain boundaries still offer higher energy barriers to diffusion. Silver, on the other hand, is not only smaller in size but, as we show for the first time, can also participate in weak bonding interactions with the host atoms where favorable geometries allow, thus reducing the energy barrier and enhancing the rate of diffusion.

Application of EPMA data for the development of the code systems TRANSURANUS and ALEPH.

In the present article, electron probe microanalysis data for Pu and Nd is being used for validating the predictions of the radial power profile in a nuclear fuel rod at an ultrahigh burn-up of 95 and 102 MWd/kgHM. As such the validation of both the new Monte Carlo burn-up code ALEPH and the simpler TUBRNP model of the fuel rod performance code TRANSURANUS has been extended. The analysis of the absolute concentrations and individual isotopes also indicates potential improvements in the predictive capabilities of the simple TUBRNP model, based on the one-group cross sections inferred from the neutron transport calculations in the ALEPH code. This is a first important step toward extending the application range of the fuel rod performance code to burn-up values projected in nuclear power rods based on current trends.